This paper describes Nd 3+-ions doped multicomponent tellurite glasses TeO2-TiO2-ZnO (TTZ) applicable to advanced optical devices, which were characterized by UV-Vis-NIR absorption, Raman, and photoluminescence (PL) techniques. Not only did we perform experimental characterizations but also theoretically predicted the PL properties of Nd 3+-doped TTZ glasses by using the Judd-Ofelt theory. The influence of the residual hydroxyl (OH) groups and types of crucible used in the melt preparation on the structures and optical properties of TTZ glasses was investigated. We found that the use of a Pt crucible increased the network-connecting structures of trigonal bipyramidal TeO4 compared to the case of a Al2O3 crucible. Moreover, reducing the OH groups in TTZ glasses improved the optical properties of Nd 3+-doped TTZ glass, and a higher spectral figure of merit of 8.71 × 10 −24 s cm 2 for Nd 3+ : 4 F3/2→ 4 I11/2 emission at 1,075 nm could be achieved, indicating that Nd 3+doped TTZ glass with lower hydroxyl content is promising for laser or active optical applications.